RSC Advances
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2022
·Vol. 12
·期 27
·17237-17248
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IF 4.036
Dongqing Feng,Jianxin Shou,Sen Guo,Mengna Ya,Jianfa Li,Huaping Dong,Yimin Li
Activation of hydrogen peroxide (H2O2) with biochar is a sustainable and low-cost approach for advanced oxidation of organic pollutants, but faces the challenge of a low yield of hydroxyl radical (˙OH). Herein, we hypothesize that the activation efficiency of H2O2 can be enhanced through co-catalysis of trace dissolved iron (Fe) with biochar. Two biochar samples derived from different feedstock, namely LB from liquor-making residue and WB from wood sawdust, were tested in the co-catalytic systems using trace Fe(III) (0.3 mg L−1). The cumulative ˙OH production in [Fe(III) + LB]/H2O2 was measured to be 3.28 times that in LB/H2O2, while the cumulative ˙OH production in [Fe(III) + WB]/H2O2 was 11.9 times that in WB/H2O2. No extra consumption of H2O2 was observed in LB/H2O2 or WB/H2O2 after addition of trace Fe(III). Consequently, the reaction rate constants (kobs) for oxidation of pollutants (2,4-dichlorophenoxyacetic acid and sulfamethazine) were enhanced by 3.13–9.16 times. Other iron species including dissolved Fe(II) and iron minerals showed a similar effect on catalyzing 2,4-D oxidation by biochar/H2O2. The interactions involved in adsorption and reduction of Fe(III) by biochar in which the defects acted as electron donors and oxygen-containing functional groups bridged the electron transfer. The fast regeneration of Fe(II) in the co-catalytic system resulted in the sustainable ˙OH production, thus the efficient oxidation of pollutants comparable to other advanced oxidation processes was achieved by using dissolved iron at a concentration as low as the concentration that can be found in natural water.
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APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Jianhui Zhu,Linchao Zeng,Xiaoya Li,Ning Zhao,Yanyi Wang,Zhilan Lin,Tingshu He,Libo Deng,Peixin Zhang
The inexpensive room-temperature sodium-sulfur (RT Na-S) battery has attracted extensive attention due to its various potential application but is still suffering from the low utilization of sulfur, the shuttle effect and the sluggish reaction activity of sodium polysulfides (SPSs). In this work, a TiO 2 /sulfur/atomic-iron loaded carbon nanosheet cathode is designed for high performance RT Na-S battery. When the atomic iron exists, a much higher electrochemical activity of sulfur was obtained, indicating the atomic iron can accelerate the conversion of SPSs. Furthermore, the TiO 2 layer can inhibit the shuttle effect of SPSs and the side-reaction between the intermediates and carbonate electrolyte. As a result, the constructed sulfur cathode exhibits a high reversible capacity (569.9 mAh g −1 with an initial coulombic efficiency of 57.57%) at 0.1 A g −1 and outstanding cycling performance (507 mAh g −1 after 50 cycles). This work provides a new strategy for preparing high performance cathode materials for RT Na-S battery.
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Journal of Environmental Chemical Engineering
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2022
·
IF 7.968
Liuqun Fan,Zhiyan Hou,Tianbao Liu,Xiangjing Liang,Andrei Ivanets,Kongjun Ma,Xintai Su
Heteroatom-doped carbon materials derived from oil-bearing sludge exhibit excellent supercapacitor performance due to their unique electronic and chemical properties. However, the complex composition of heteroatoms in oil-bearing sludge makes it difficult to achieve sufficient and directional doping by direct pyrolysis . In this paper, an oleic acid pretreatment-roasting-secondary activation strategy was developed to make full use of hydrocarbons, iron- and nitrogen-containing compounds in oil-bearing sludge to prepare Fe-N X -C materials with excellent electrochemical properties. Characterization results such as transmission electron microscopy (TEM) and N 2 adsorption analysis showed that the best sample had a hierarchical pore structure and uniform Fe and N element loading. X-ray photoelectron spectroscopy (XPS) analysis found that the addition of oleic acid can promote the formation of Fe-Nx, and the dosage of oleic acid will affect the content of Fe-Nx in the carbon materials. Electrochemical characterization of this supercapacitor material was conducted. The best sample's specific capacitance was as high as 293.6 F g −1 at the current density of 0.5 A g −1 , and the capacitance retention rate could still reach 71.5% at the current density of 10 A g −1 . The assembled button-type symmetrical supercapacitors had an energy density of 8.68 Wh kg −1 and a power density of 137.53 W kg −1 , which is much higher than those of most other waste-based carbon materials. This work presents a new idea for the preparation of heteroatom doped carbon materials with excellent capacitive properties from oily sludge, which provides a new reference for the treatment and resource utilization of oily sludge.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2022
·
IF 5.518
Zihao Hu,Beiyang Guo,Huiqi Wu,Fang Zhu,Sridhar Komarneni,Jianfeng Ma
In this paper, MIL-101(Fe) and MoS 2 composites (MIL-101(Fe)/MoS 2 ) were synthesized using a facile solvothermal method . As a new degradation system, the synthesized composites were investigated using persulfate (PS) activation based on visible light (Vis). To establish the superiority of a heterogeneous photochemical catalysis system, the MIL-101(Fe)/MoS 2 was used as the catalyst in the presence of Na 2 S 2 O 8 with visible light irradiation. In the system mentioned, the MIL-101(Fe)/MoS 2 catalyst presented a much better catalytic ability than that of either a single photocatalysis or chemocatalysis system. The better catalytic ability suggests that the MIL-101(Fe)/MoS 2 catalyst was capable of effectively integrating photocatalysis and chemocatalysis leading to the highest degradation efficiency of 85% in 40 min with tetracycline as the target pollutant. The catalytic system MIL-101(Fe)/MoS 2 /PS/Vis degraded TC pollutant by forming species of O 2 ‾, 1 O 2 , hydroxyl radicals (•OH) and sulfate radicals (•SO 4 ‾) to degrade TC. Furthermore, the MIL-101(Fe)/MoS 2 catalyst displayed better catalytic performance compared to those materials that were previously reported, as verified by the good stability (reached 80% after three cycles) and the high TC degradation rate (85%) of the currently developed material. This system may be applicable to the degradation of TC and other challenging organic pollutants .
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
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2022
·Vol. 30
·期 1
·1399-1412
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IF 5.19
Chen Jun,Zhang Boding,Wang Bingxing,Zhang Wenlong,Wang Jichao,Cui Chengxing,Wang Songlin
Wastewater containing quinoline has become a common pollutant in water and soil environments, which poses a threat to human health due to its carcinogenicity, teratogenicity, and mutagenicity. Quinoline’s stability and toxicity hinders its degradation by conventional physicochemical and biological methods. In this contribution, Fe-Co-Bi/kaolin particle electrodes were prepared for the efficient degradation of quinoline in wastewater, and characterized by using scanning electron microscope, X-ray diffraction, pyridine-IR, Brunauer–Emmett–Teller, X-ray photoelectron spectroscopy, and four-probe resistivity test. Parameters affecting the degradation efficiency were optimized to be the particle electrode dosage of 40 g/L, pH 3.5, H 2 O 2 addition of 67.6 mmol/L, electrical conductivity of 12.7 ms/cm, and voltage of 20 V. The constructed three-dimensional catalytic particle electrode system (3D-CPE) achieved 92.1% removal rate of chemical oxygen demand (COD) under the optimal conditions. Hydroxyl radicals (•OH) generated in the 3D-CPE process were identified by radical scavenging tests and electron spin response analysis. To unravel the degradation mechanism, the intermediate products were identified by using high performance liquid chromatography-mass spectrometry. The degradation mechanism was discussed with the help of theoretical calculation.
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ANALYTICAL AND BIOANALYTICAL CHEMISTRY
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2022
·Vol. 414
·期 26
·7741-7751
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IF 4.478
Liu Yuqian,Hu Xianyun,Liang Fangyuan,Cao Yajing
Exploring sensors based on Förster resonance energy transfer (FRET) systems enables the continuous development of biological sensing technologies. Herein, we report the construction of a FRET sensor with dual-emissive quantum dots (QDs) and meso -tetra(4-sulfonatophenyl) porphine (TSPP). The sensor is composed of mesial green-emissive QDs with a thick silica shell (gQD@SiO 2 ) and circumjacent blue-emissive QDs coated with ultra-thin silica spacer, on which is linked TSPP (bQD@SiO 2 -TSPP). The gQD@SiO 2 endows the sensor with a fluorescent background. Due to the ultra-thin silica spacing, coupled with the superior resonance effect of bQD fluorescence and the Soret-band absorption of TSPP, the FRET efficiency is highly sensitive to the chelation state of TSPP. Relying on the absorbance transition of TSPP complexed with Fe(III), the FRET sensor is applied for ultra-sensitive Fe(III) detection. In aqueous solution, the sensor is demonstrated to linearly detect Fe(III) in the range of 0–1 μM, with a limit of detection (LOD) of 40 nM. More importantly, reliable Fe(III) detection can be achieved via the specific complexation of Fe(III) by TSPP and the ratiometric fluorescent response. As such, the inter-/intra-day precisions in standard samples, as well as the recovery rate in biological matrices, are fully validated. The excellent analytical performance, in combination with the excellent biocompatibility of the FRET sensor, allows semi-quantitative Fe(III) imaging in living cells. Graphical abstract
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Green Energy & Environment
·
2021
·
IF 8.207
Ruichang Xue,Mengwei Guo,Zhuoming Wei,Qibo Zhang
Ni–Fe bimetallic electrodes are currently recognized as a kind of benchmark transition metal-based oxygen evolution reaction (OER) electrocatalysts. Facile synthesis of Ni–Fe bimetallic electrode materials with excellent catalytic activity and satisfied stability by a simple and low-cost route is still a big challenge. Herein, well-defined Ni–Fe nanoparticles in-situ developed on a planar Fe substrate (Ni–Fe NPs/Fe) is fabricated via a facile one-step galvanic replacement reaction (GRR) carried out in an Ethaline-based deep eutectic solvent (DES). The prepared Ni–Fe NPs/Fe exhibits outstanding OER performance, which needs an overpotential of only 319 mV to drive a current density of 10 mA cm −2 , with a small Tafel slope of 41.2 mV dec −1 in 1.0 mol L −1 KOH, high mass activity (up to 319.78 A g −1 at an overpotential of 300 mV) and robust durability for 200 h. Impressively, the Ni–Fe bimetallic oxygen-evolution electrode obtained from the Ethaline-based DES is catalytically more active and durable than that of its counterpart derived from the 4.2 mol L −1 NaCl aqueous solution. The reason for this is mainly related to the different morphology and surface state of the Ni–Fe catalysts obtained from these different solvent environments, particularly for the differences in phy–chemical properties, active species formed and deposition kinetics, offered by the Ethaline-based DES.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2021
·
IF 8.128
Zhendong Yu,Jiachen Ma,Xiaoyi Huang,Yuancai Lv,Yifan Liu,Chunxiang Lin,Rongni Dou,Xiaoxia Ye,Yongqian Shi,Minghua Liu
In this study, the S modified iron-based catalyst (S-Fe@C) for activating peroxydisulfate (PDS) was fabricated by heating the S-MIL-101 (Fe) precursor at 800 °C. The resulted S-Fe@C composite mainly consisted of carbon, Fe 0 , FeS, FeS 2 , and Fe 3 O 4 , and showed strong magnetism. Compared with Fe@C obtained from MIL-101 (Fe), the S-Fe@C exhibited much higher performance (1.5 times larger) on PDS activation and the S-Fe@C/PDS could rapidly degrade various organic pollutants in 5 min under the attack of the species of SO 4 - · , 1 O 2 , electro-transfer and Fe(IV). The S element in enhancing the PDS activation mainly involved two mechanisms. Firstly, the doped S could speed up the electron transfer efficiency, resulting in a promotion on PDS decomposition; secondly, the S 2- S 2 2- or S 0 could achieve the circulation of Fe 2+ and Fe 3+ , leading to the formation of non-radicals Fe(IV) and 1 O 2 .
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2021
·
IF 19.503
Pijun Duan,Jingwen Pan,Weiyan Du,Qinyan Yue,Baoyu Gao,Xing Xu
Cheap and abundant Fe based catalysts in advanced oxidation progresses (AOPs) usually exhibit radicals or high-valent Fe species (HV-Fe) dominated activation mechanism. In this contribution, the atomically dispersed Fe on g-C 3 N 4 (SAFe-CN) was fabricated for peroxymonosulfate (PMS) activation to degrade o-phenylphenol (OPP). OPP removal was not impeded by common radical scavengers, indicating the absence of SO 4 •− and •OH. The involvement of 1 O 2 and HV–Fe was excluded and the mediated electron transfer was finally identified as the dominated mechanism. Atomically dispersed Fe sites in SAFe-CN were verified as active sites for reacting with O O bond of PMS and ulteriorly electron shuttling in pollutants degradation. A water treatment filter was fabricated using SAFe-CN and it remained 100% of OPP removal after 100 h of operation. These results provide new insights into the mechanism of mediated electron transfer as well as potential application of non-radical dominated process at device level.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2021
·
IF 19.503
Libo Deng,Lei Qiu,Rong Hu,Lei Yao,Zijian Zheng,Xiangzhong Ren,Yongliang Li,Chuanxin He
Single-atom catalysts (SAC) stabilized by nitrogen in carbon support are promising candidates for oxygen reduction reaction (ORR). However, conventional preparation methods usually lead to encapsulation of metallic centers in matrix and thus the utilization efficiency (UE) is underexploited. Herein, we report a novel strategy to prepare an Fe-SAC with all Fe atoms anchored on the surface of carbon nanospheres , which exhibited an extraordinary UE of 80% for ORR. This efficiency was achieved by coating polydopamine spheres with silica, followed by the pyrolysis of their blend with FeCl 3 . During thermal treatment, Fe migrates across the silica shell by atomic exchange with silicon, which inhibits the aggregation of Fe and allows Fe atoms to anchor on the surface. As such, it showed excellent ORR activity at a low Fe content. Zn-air batteries assembled using this catalyst showed a peak power density of 113 mW cm −2 and specific capacity of 710 mAh g Zn −1 .
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MATERIALS LETTERS
·
2021
·
IF 3.423
Y.G. Wang,M. Wang,Y.Q. Wang,Q. Zhang,H.N. Zhou,H.L. Zhao
Prussian green (PG) film was directly grown on FTO glass by one-step hydrothermal process for excellent electrochromic performance. The electrochromic devices (ECDs) based on as-grown PG film can show reversible color changes between green, blue and colorless states. The existence state of iron elemental in PG film at different color states was studied by X-ray photoelectron spectroscopy. Compared with the traditional Prussian blue ECDs, PG ECDs achieve a higher optical modulation range (42.7%) and a shorter switching time (t c /t b =1.0/7.4 s). This study provides a novel method for preparing high-performance three-color ECDs by a simple hydrothermal method, and clearly shows the evolution of Fe ions during the discoloration process.
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ELECTROCHIMICA ACTA
·
2021
·
IF 6.901
Chen Hou,Yi-Ran Xing,Le-Le Yu,Yong-Heng Si,Han Lu,Yu-Juan Zhao
Fe–Mn based Li-rich cathode materials are regarded as one of the most promising cathode materials for their low cost and high energy density but possess drawbacks such as high oxygen release, low conductivity, and slow kinetics for lithium-ion transport. To address these issues, herein, we proposed a high-valance cations Nb 5+ doping strategy and synthesized a series of Li 1.26 [Fe 0.22 Mn 0.52 ] 1−x Nb 0.74x O 2 ( x = 0, 0.02, 0.03, 0.04) cathode materials. Using a combination of experimental approaches and density functional theory (DFT) calculations, we found that the doped samples presented expanded interlayer spacing for Li-ion migration and better structural stability due to the large ionic radius of Nb 5+ and the strengthened Nb–O bond. Moreover, Nb doping could not only decrease the band gap and the density of states of the O 2p band but also contribute extra electrons to surrounding O atoms, thereby enhancing electronic conductivity and stabilizing lattice oxygen. Benefit from the underlying mechanisms mentioned above, the Nb 0.022 sample possessed a higher Coulombic efficiency (71.1 vs 65.0%) at 0.2 C, showing more stable cycling performance (90.4 vs 67.7 mAh g −1 ) at 0.5 C and rate capability. These favorable results can assist in the development of Fe–Mn based Li-rich cathode materials with excellent electrochemical properties.
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